Sorption-enhanced steam reforming of glycerol (SESRG) is a promising method for the sustainable production of hydrogen (H-2). In this work, composites of Ni and cationic-modified hydrotalcite (HTlc) were promoted with Pt, thus resulting in two novel hybrid materials Pt-NiMgHTlc and Pt-NiCuHTlc. Activity trials for SESRG were performed in a fixed-bed reactor in the range 673-873K and it was found that the promotion with Pt improved H-2 purity and multi-cycle durability. The best results were achieved when Pt-NiCuHTlc was employed at T = 823 K: a H-2 concentration of 98.7 mol% and adsorption capacity of 1.34 mol CO2/kg sorbent was achieved. When the multi-cycle performance was tested for 20 cycles, it was found that NiMgHTlc, NiCuHTlc, Pt-NiMgHTlc, and Pt-NiCuHTlc were stable for 5, 8, 13, and 18 cycles. Finally, a likely reaction pathway for SESRG over the investigated multifunctional materials was proposed.